Adhesion and delamination have been pervasive problems hampering the performance and reliability of micro-and nano-electronic devices. In order to understand, predict, and ultimately prevent interface failure in electronic devices, development of accurate, robust, and efficient delamination testing and prediction methods is crucial. Adhesion is essentially a multi-scale phenomenon: at the smallest scale possible, it is defined by the thermodynamic work of adhesion. At larger scales, additional dissipative mechanisms may be active which results in enhanced adhesion at the macroscopic scale and are the main cause for the mode angle dependency of the interface toughness. Undoubtedly, the macroscopic adhesion properties are a complex function of all dissipation mechanisms across the scales. Thorough understanding of the significance of each of these dissipative mechanisms is of utmost importance in order to establish physically correct, unambiguous, values of the adhesion properties, which can only be achieved by proper multi-scale techniques. The topic “Advances in Delamination Modeling” has been split into two separate chapters: this chapter discusses the atomistic aspects of delamination, while the preceding chapter deals with the atomistic aspects of interface separation. The chapter starts with a concise overview of molecular simulation strategies. Next, examples are provided which represent actual materials being developed for electronic packaging: (1) the prediction of thermomechanical properties of an epoxy molding compound (EMC) and the adhesion properties of an EMC/copper interface by means of MD and CG MD approaches; (2) the modeling of wetting, adhesion, and reliability cycling of die attach and via fills; (3) model scaling to discrete element modeling (DEM) for understanding underfill flow; (4) CG modeling of an epoxy molding compound which relates to the first example; (5) molecular modeling of silicate layers used in planarization and encapsulant layers for flat panel displays; (6) mesoscale modeling of diffusion of organic bases which is of concern to photoresist poisoning; and (7) the prediction of thermomechanical properties of a low-k dielectric material, SiOC:H.